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Phys. Rev. Lett. 89, 237401 (2002) [4 pages]

Correlated Vibrational Dynamics Revealed by Two-Dimensional Infrared Spectroscopy

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N. Demirdöven, M. Khalil, and A. Tokmakoff
Department of Chemistry, Massachusetts Institute of Technology, Cambridge, Massachusetts 02139

Received 14 June 2002; published 15 November 2002

Two-dimensional infrared (2D IR) spectroscopy has been used to monitor the solvent-induced correlated fluctuations in the transition energies of two coupled vibrations. The elongation of diagonal and cross peaks in a 2D IR correlation spectrum reflects the degree of inhomogeneity in the individual transition energies and the correlation between them. Changes in the 2D line shapes as a function of a variable waiting period have been successfully reproduced by a correlated spectral diffusion model.

© 2002 The American Physical Society

URL:
http://link.aps.org/doi/10.1103/PhysRevLett.89.237401
DOI:
10.1103/PhysRevLett.89.237401
PACS:
78.30.Jw, 42.50.Md, 63.50.+x, 78.47.+p